Size-dependent kinetics during non-equilibrium lithiation of nano-sized zinc ferrite

Jing Li, Qingping Meng, Yiman Zhang, Lele Peng, Guihua Yu, Amy C. Marschilok, Lijun Wu, Dong Su, Kenneth J. Takeuchi, Esther S. Takeuchi, Yimei Zhu and Eric A. Stach ()
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Jing Li: SUNY-Stony Brook University
Qingping Meng: Brookhaven National Laboratory
Yiman Zhang: SUNY-Stony Brook University
Lele Peng: The University of Texas at Austin
Guihua Yu: The University of Texas at Austin
Amy C. Marschilok: SUNY-Stony Brook University
Lijun Wu: Brookhaven National Laboratory
Dong Su: Brookhaven National Laboratory
Kenneth J. Takeuchi: SUNY-Stony Brook University
Esther S. Takeuchi: SUNY-Stony Brook University
Yimei Zhu: Brookhaven National Laboratory
Eric A. Stach: University of Pennsylvania

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract Spinel transition metal oxides (TMOs) have emerged as promising anode materials for lithium-ion batteries. It has been shown that reducing their particle size to nanoscale dimensions benefits overall electrochemical performance. Here, we use in situ transmission electron microscopy to probe the lithiation behavior of spinel ZnFe2O4 as a function of particle size. We have found that ZnFe2O4 undergoes an intercalation-to-conversion reaction sequence, with the initial intercalation process being size dependent. Larger ZnFe2O4 particles (40 nm) follow a two-phase intercalation reaction. In contrast, a solid-solution transformation dominates the early stages of discharge when the particle size is about 6–9 nm. Using a thermodynamic analysis, we find that the size-dependent kinetics originate from the interfacial energy between the two phases. Furthermore, the conversion reaction in both large and small particles favors {111} planes and follows a core-shell reaction mode. These results elucidate the intrinsic mechanism that permits fast reaction kinetics in smaller nanoparticles.

Date: 2019
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DOI: 10.1038/s41467-018-07831-5

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